EP1187153A1 - Polarisierbare elektrode für elektrische doppellagen-kapazität - Google Patents

Polarisierbare elektrode für elektrische doppellagen-kapazität Download PDF

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Publication number
EP1187153A1
EP1187153A1 EP01917482A EP01917482A EP1187153A1 EP 1187153 A1 EP1187153 A1 EP 1187153A1 EP 01917482 A EP01917482 A EP 01917482A EP 01917482 A EP01917482 A EP 01917482A EP 1187153 A1 EP1187153 A1 EP 1187153A1
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EP
European Patent Office
Prior art keywords
double layer
polarizable electrode
electrical double
sheet
layer capacitors
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Granted
Application number
EP01917482A
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English (en)
French (fr)
Other versions
EP1187153B1 (de
EP1187153A4 (de
Inventor
Tomohiro Bogaki
Masashi NGK INSULATORS LTD. ONO
Toshihiko NGK INSULATORS LTD. NAKAGAWA
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NGK Insulators Ltd
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NGK Insulators Ltd
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Publication date
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Publication of EP1187153A1 publication Critical patent/EP1187153A1/de
Publication of EP1187153A4 publication Critical patent/EP1187153A4/de
Application granted granted Critical
Publication of EP1187153B1 publication Critical patent/EP1187153B1/de
Anticipated expiration legal-status Critical
Expired - Lifetime legal-status Critical Current

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
    • H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
    • H01G11/22—Electrodes
    • H01G11/26—Electrodes characterised by their structure, e.g. multi-layered, porosity or surface features
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
    • H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
    • H01G11/22—Electrodes
    • H01G11/30—Electrodes characterised by their material
    • H01G11/32—Carbon-based
    • H01G11/38—Carbon pastes or blends; Binders or additives therein
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
    • H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
    • H01G11/66—Current collectors
    • H01G11/72—Current collectors specially adapted for integration in multiple or stacked hybrid or EDL capacitors
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/96—Carbon-based electrodes
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/13—Energy storage using capacitors
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells

Definitions

  • the present invention relates to a polarizable electrode for use in electrical double layer capacitors.
  • the present invention has been achieved in view of the fact that the conventional technologies have such problems, and thus has an object to provide a polarizable electrode for use in electrical double layer capacitors, which polarizable electrode can reduce the long-term performance degradation and self-discharge caused energy losses of the electrical double layer capacitors, by suppressing the dropped carbon particles when the polarizable electrode is impregnated with an electrolytic solution.
  • a polarizable electrode for use in electrical double layer capacitors which polarizable electrode comprises carbon fine-powder, a conductive auxiliary agent, and a binder, and which is characterized in that the tensile strength of the above described polarizable electrode is not less than 0.13 MPa.
  • the dropped particle amount of the carbon particles leaving into the electrolytic solution is preferably not more than 1.0 mg/cm 2 .
  • Fig. 1 shows a flaw chart illustrating an example of a method of manufacturing a polarizable electrode according to the invention.
  • Fig. 2 shows a schematic representation of a kneader used in the present invention.
  • Fig. 3 shows a schematic representation of a roll-pressing machine used in the present invention.
  • Fig. 4 shows a schematic representation of a rolling machine (reduction roller) used in the present invention.
  • Fig. 5 shows a schematic diagram of electrical double layer capacitors in the examples 1 to 3 and a comparative example 1.
  • the polarizable electrode of the present invention is a polarizable electrode for use in electrical double layer capacitors which comprises carbon fine-powders, a conductive auxiliary agent, and a binder, and which has tensile strength of not less than 0.13 MPa.
  • the polarizable electrode when the polarizable electrode is impregnated with an electrolytic solution, the dropped carbon particles contained in the polarizable electrode can be suppressed, so that it is possible to reduce the long-term performance degradation and self-discharge caused energy losses of the electrical double layer capacitors.
  • the dropped particle amount of the carbon particles leaving from the polarizable electrode into the electrolytic solution is preferably not more than 1.0 mg/cm 2 .
  • the dropped particle amount of the carbon particles is more than 1.0 mg/cm 2 , the carbon particles suspended in the electrolytic solution become large in number, and therefore the self-discharge rate of the electrical double layer capacitor becomes high when it is in practical use, thereby resulting in the degradation of long-term performance of the electrical double layer capacitor.
  • the polarizable electrode of the invention can make the self-discharge rate of the electrical double layer capacitor not more than 10%, the energy losses thereof can be reduced.
  • the carbon fine-powder used in the invention can adsorb anions and cations existing in the electrolytic solution to form an electrical double layer, thus serving for storage of electrical power.
  • the conductive auxiliary agent used in the invention increase the electrical conductivity between the carbon fine-powders themselves and between the carbon powders and the collector.
  • the mixing ratio of the carbon fine-powder plays important role for increasing energy density per unit area in the polarizable electrode, and the mixing ratio of the conductive auxiliary agent exerts influence on the internal resistance of the polarizable electrode to contribute to improvement in the output density.
  • the mixing ratio of the conductive auxiliary agent should be adjusted in accordance with the intended use of the polarizable electrode.
  • the mixing ratio of the conductive auxiliary agent is 3 to 10 weight parts relative to 100 weight parts of carbon fine-powder.
  • the mixing ratio of the conductive auxiliary agent is preferably 8 to 20 weight parts relative to 100 weight parts of carbon fine-powder.
  • a mixture comprising a conductive auxiliary agent of 3 to 20 weight parts relative to 100 weight parts of carbon fine-powder is suitably used.
  • the mixing ratio of the conductive auxiliary agent is more than 20 weight parts, the internal resistance can be little decreased and the mixing ratio of the carbon fine-powder contained in unit volume decreases conversely, thereby resulting in decreased energy density.
  • the binder used in the invention is preferably a fluorine resin, and for example, the binder described in Japanese Patent Publication No. 7-44127 can be suitably used.
  • polytetrafluoroethylene ethylene-tetorafluoroethylene copolymer, ethylene-chlorotrifluoroethylene, vinyliden fluoride copolymer, tetrafluoroethylene-perphloroalkylenevinylether copolymer etc.
  • PTFE polytetrafluoroethylene
  • ethylene-tetorafluoroethylene copolymer ethylene-chlorotrifluoroethylene
  • vinyliden fluoride copolymer tetrafluoroethylene-perphloroalkylenevinylether copolymer etc.
  • the tetorafluoroethylene can be suitably used because it is chemically stable.
  • the mixing ratio of the above fluorine resin is preferably 3 to 15 weight parts (more preferably 5 to 10 weight parts) relative to 100 weight parts of carbon fine-powder.
  • Fig. 1 is a flowchart illustrating one example of a method of manufacturing the polarizable electrode of the present invention.
  • carbon powder prepared by adding a conductive auxiliary agent of the amount of 3 to 20 weight parts to 100 weight parts of a predetermined amount of carbon fine-powder, and a binder made of a fluorine resin are mixed together such that they may be uniformly dispersed (raw materials mixing process).
  • the mixing is preferably performed at temperature not higher than the transition temperature of the fluorine resin (in the case of PTFE, at 19°C and below).
  • the mixture obtained in the raw materials mixing process is sufficiently kneaded while heated at temperature between 20 and 120°C and subjected to shearing force, for example, by means of a kneader shown in Fig. 2 (kneading process).
  • the fluorine resin of the binder has fine fiber-like structures, which are bound to each other so as to form kneaded material consisting of small piece clusters having small bulk density and apparent volume of about 0.01 to 10 cm 3 .
  • the kneading temperature may be a temperature at which the fluorine resin exhibits enough flawability (for example, 50°C), and may be sufficient up to about 120°C.
  • the applied shearing force and the time of kneading are adequate, provided that each of the materials can be sufficiently and uniformly kneaded with each other.
  • liquid lubricant may be added in order to facilitate fibrous growth of the binder.
  • the kneaded material obtained in the kneading process is formed into a sheet-like compact of a predetermined thickness (for example, 0.3 mm), for example, by means of a roll press machine (sheet forming process).
  • the above sheet-like compact can be strengthened by partial binding between the finely fibrous structures which have been formed of the fluorine resin, by which carbon powder can be fixed more firmly.
  • the sheet-like compact obtained in the sheet forming process can be used as a polarizable electrode even as it is.
  • the sheet-like compact is rolled until a predetermined thickness (for example, 0.2 mm) is reached, for example, by means of a rolling machine (reduction roller) shown in Fig. 4, thereby polarizable-electrode sheets for use in capacitors being formed.
  • this sheet is cut to a predetermined size, thereby intended polarizable electrodes for use in capacitors being obtained.
  • the sheets for use in polarizable electrodes and the electrical double layer capacitors obtained in each example were evaluated in performance by the following methods.
  • the polarizable-electrode sheets were stamped with a punch etc. into sheets of the shape of ⁇ 19 mm, which were dried sufficiently and then the initial weight W1 thereof was determined.
  • this sheet was taken out of the acetonitrile and dried, and then the post-impregnation weight W2 was determined.
  • Powdered activated-carbon 80%, carbonblack 10%, and polytetrafluoroethylene (PTFE) 10% were weighed, and sufficiently mixed together with water of the same weight as the solid matter, and then kneaded at 50°C for 10 minutes by means of a kneader. After that, the kneaded material was shaped through a roll forming machine into a polarizable electrode sheet of 150 ⁇ m thick.
  • PTFE polytetrafluoroethylene
  • a polarizable electrode 42 was brought into intimate contact with the surface of aluminum foil of a collecting electrode 40, and two sets of these were placed such that the polarizable electrodes 42 thereof could be opposed to each other. Then, a separator 44 made of cellulose was inserted between the polarizable electrodes 42, which then were impregnated with an electrolytic solution 48 that was a propylene carbonate solution of 1M boron 4-ethyl ammonium 4-fluoride, thereby forming a electrical double layer capacitor (refer to see Fig. 5).
  • PTFE polytetrafluoroethylene
  • Powdered activated-carbon 85%, carbonblack 10% and polytetrafluoroethylene (PTFE) 5% were weighed and sufficiently mixed together with water of the same weight as the solid matter, and then kneaded at 50°C for 20 minutes by means of a kneader. After that, the kneaded material was shaped through a roll forming machine into a sheet of 150 ⁇ m thick.
  • PTFE polytetrafluoroethylene
  • PTFE polytetrafluoroethylene
  • the dropped particle amount of the carbon particles leaving into the electrolytic solution can be made not more than 1.0 mg/cm 2 and the self-discharge rate of the electrical double layer capacitors in practical can be made not higher than 10%, by making the tensile strength of the polarizable electrodes not less than 0.13 MPa.
  • the polarizable electrode for use in electrical double layer capacitors allows reduction of long-term performance degradation and self-discharge caused energy losses of the electrical double layer capacitor, by suppressing the dropped the carbon powders contained in the polarizable electrode when it is impregnated with an electrolytic solution.

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  • Engineering & Computer Science (AREA)
  • Power Engineering (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • Chemical & Material Sciences (AREA)
  • Materials Engineering (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Electric Double-Layer Capacitors Or The Like (AREA)
EP01917482A 2000-03-22 2001-03-21 Polarisierbare elektrode für elektrischen doppelschichtkondensator Expired - Lifetime EP1187153B1 (de)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
JP2000080818A JP2001267187A (ja) 2000-03-22 2000-03-22 電気二重層コンデンサ用分極性電極
JP2000080818 2000-03-22
PCT/JP2001/002238 WO2001071739A1 (en) 2000-03-22 2001-03-21 Polarizable electrode for electric double-layer capacitor

Publications (3)

Publication Number Publication Date
EP1187153A1 true EP1187153A1 (de) 2002-03-13
EP1187153A4 EP1187153A4 (de) 2005-08-03
EP1187153B1 EP1187153B1 (de) 2007-09-19

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EP01917482A Expired - Lifetime EP1187153B1 (de) 2000-03-22 2001-03-21 Polarisierbare elektrode für elektrischen doppelschichtkondensator

Country Status (5)

Country Link
US (1) US6614646B2 (de)
EP (1) EP1187153B1 (de)
JP (1) JP2001267187A (de)
DE (1) DE60130528T2 (de)
WO (1) WO2001071739A1 (de)

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Publication number Publication date
DE60130528D1 (de) 2007-10-31
EP1187153B1 (de) 2007-09-19
WO2001071739A1 (en) 2001-09-27
EP1187153A4 (de) 2005-08-03
US20020181186A1 (en) 2002-12-05
US6614646B2 (en) 2003-09-02
DE60130528T2 (de) 2008-06-12
JP2001267187A (ja) 2001-09-28

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